CN111315474A - Flow type reaction device - Google Patents

Flow type reaction device Download PDF

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Publication number
CN111315474A
CN111315474A CN201880071998.0A CN201880071998A CN111315474A CN 111315474 A CN111315474 A CN 111315474A CN 201880071998 A CN201880071998 A CN 201880071998A CN 111315474 A CN111315474 A CN 111315474A
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China
Prior art keywords
mixer
raw material
gas
liquid
supply
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CN201880071998.0A
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Chinese (zh)
Inventor
酒井和也
德冈慎也
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Taiyo Nippon Sanso Corp
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Taiyo Nippon Sanso Corp
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B35/00—Boron; Compounds thereof
    • C01B35/02—Boron; Borides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
    • B01F23/20—Mixing gases with liquids
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
    • B01F23/20—Mixing gases with liquids
    • B01F23/23—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids
    • B01F23/232—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids using flow-mixing means for introducing the gases, e.g. baffles
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F23/00—Mixing according to the phases to be mixed, e.g. dispersing or emulsifying
    • B01F23/20—Mixing gases with liquids
    • B01F23/23—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids
    • B01F23/232—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids using flow-mixing means for introducing the gases, e.g. baffles
    • B01F23/2323—Mixing gases with liquids by introducing gases into liquid media, e.g. for producing aerated liquids using flow-mixing means for introducing the gases, e.g. baffles by circulating the flow in guiding constructions or conduits
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F25/00—Flow mixers; Mixers for falling materials, e.g. solid particles
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F25/00—Flow mixers; Mixers for falling materials, e.g. solid particles
    • B01F25/30—Injector mixers
    • B01F25/31—Injector mixers in conduits or tubes through which the main component flows
    • B01F25/314—Injector mixers in conduits or tubes through which the main component flows wherein additional components are introduced at the circumference of the conduit
    • B01F25/3143—Injector mixers in conduits or tubes through which the main component flows wherein additional components are introduced at the circumference of the conduit characterised by the specific design of the injector
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J10/00—Chemical processes in general for reacting liquid with gaseous media other than in the presence of solid particles, or apparatus specially adapted therefor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
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    • B01J19/002—Avoiding undesirable reactions or side-effects, e.g. avoiding explosions, or improving the yield by suppressing side-reactions
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    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/2415—Tubular reactors
    • B01J19/243—Tubular reactors spirally, concentrically or zigzag wound
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B6/00—Hydrides of metals including fully or partially hydrided metals, alloys or intermetallic compounds ; Compounds containing at least one metal-hydrogen bond, e.g. (GeH3)2S, SiH GeH; Monoborane or diborane; Addition complexes thereof
    • C01B6/06—Hydrides of aluminium, gallium, indium, thallium, germanium, tin, lead, arsenic, antimony, bismuth or polonium; Monoborane; Diborane; Addition complexes thereof
    • C01B6/10—Monoborane; Diborane; Addition complexes thereof
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01F—MIXING, e.g. DISSOLVING, EMULSIFYING OR DISPERSING
    • B01F2101/00—Mixing characterised by the nature of the mixed materials or by the application field
    • B01F2101/2204—Mixing chemical components in generals in order to improve chemical treatment or reactions, independently from the specific application
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    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00159—Controlling the temperature controlling multiple zones along the direction of flow, e.g. pre-heating and after-cooling
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00162—Controlling or regulating processes controlling the pressure
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    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
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    • B01J2219/00049—Controlling or regulating processes
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    • B01J2219/00889—Mixing
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    • B01J2219/0095—Control aspects
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    • B01J2219/19—Details relating to the geometry of the reactor
    • B01J2219/194—Details relating to the geometry of the reactor round
    • B01J2219/1941—Details relating to the geometry of the reactor round circular or disk-shaped
    • B01J2219/1944—Details relating to the geometry of the reactor round circular or disk-shaped spiral

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  • Chemical & Material Sciences (AREA)
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  • Inorganic Chemistry (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

The present invention addresses the problem of providing a flow reactor (1) for continuously reacting two or more raw material substances, which can maintain reaction efficiency and productivity sufficient for practical use for a long period of time and can achieve reduction in size and cost of a reaction facility, and which comprises: a mixing section (10) for mixing two or more raw material substances; and a reaction section (20) which is provided on the secondary side of the mixing section (10) and which obtains a product by reacting the raw material substances, wherein the mixing section (10) has: a mixer (13) for mixing two or more of the raw material substances; and two or more supply paths (L11, L12) for supplying the respective raw material substances to the mixer (13), wherein the supply paths (L11, L12) are connected to the mixer (13), respectively, and the supply path (L11) has a suppression mechanism that suppresses the movement of the fluid from the mixer (13) to the supply path (L11) in the vicinity of the connection portion between the supply path (L11) and the mixer (13).

Description

Flow type reaction device
Technical Field
The present invention relates to a flow-type reaction apparatus. The present application claims priority based on patent application No. 2017-233618, filed in japan, 12/5/2017, and the contents of which are incorporated herein by reference.
Background
Attention is being paid to a flow-type reaction apparatus for continuously supplying a raw material to a reaction field and causing a continuous chemical reaction. The flow-type reaction apparatus has advantages such as being capable of producing a target substance with high production efficiency, being capable of artificially controlling a chemical reaction, being small-sized and safe in reaction equipment, and the like, as compared with a so-called batch-type reaction apparatus.
However, the flow-type reaction apparatus has the following problems: that is, a supply pipe for supplying the raw material to the reaction field is easily clogged due to a solid or the like generated as a by-product in the chemical reaction. Accordingly, patent documents 1 to 3 disclose techniques for coping with the clogging.
Patent document 1: japanese patent laid-open No. 2012-228666
Patent document 2: japanese patent laid-open publication No. 2004-344877
Patent document 3: japanese patent laid-open No. 2006-181525
However, in the apparatuses described in patent documents 1 to 3, when sudden pressure fluctuations occur in the reaction field due to the progress of the chemical reaction, liquid backflow frequently occurs in the apparatuses. And due to this backflow, the liquid adheres to the supply line and causes precipitation of solids, resulting in clogging of the supply line.
Therefore, in the apparatuses disclosed in patent documents 1 to 3, when the apparatuses are operated for a long time, the supply lines and the like are clogged due to the backflow, and the raw materials cannot be supplied to the reaction field. Therefore, the apparatuses disclosed in patent documents 1 to 3 have a reduced reaction efficiency with the progress of the chemical reaction, and cannot ensure a sufficient operating time and high productivity for practical use. In addition, since the reaction efficiency is lowered, unreacted raw material substances are mixed into the final product, and the quality such as purity of the target substance is lowered.
The device described in patent document 1 is not suitable for downsizing and cost reduction of a reaction apparatus because it requires an ultrasonic transducer for applying ultrasonic vibration to a supply line.
Disclosure of Invention
The present invention has been made in view of the above circumstances, and an object of the present invention is to provide a flow reactor capable of maintaining reaction efficiency and productivity sufficient for practical use and realizing reduction in size and cost of a reaction facility.
In order to solve the above problems, the present invention provides the following flow reactor.
[1] A flow-type reaction apparatus for continuously reacting two or more kinds of raw material substances, comprising: a mixing section for mixing two or more of the raw material substances; and a reaction section provided on a secondary side of the mixing section and obtaining a product by reacting the raw material substances, the mixing section including: a mixer for mixing two or more of the raw material substances; and two or more supply lines for supplying the respective raw material substances to the mixer, the supply lines being connected to the mixers, respectively, and at least one of the supply lines having a suppression mechanism in the vicinity of a connection portion between the supply line and the mixer, the suppression mechanism suppressing movement of a fluid from the mixer to the supply line.
[2] A flow-type reaction apparatus for continuously reacting two or more kinds of raw material substances, comprising: a mixing section for mixing two or more of the raw material substances; and a reaction section provided on a secondary side of the mixing section and obtaining a product by reacting the raw material substances, the mixing section including: a mixer for mixing two or more of the raw material substances; and two or more supply pipes for supplying the respective raw material substances to the mixers, the supply pipes being connected to the mixers, respectively, and at least one of the supply pipes being connected to the mixer from above with respect to a plane in which the mixer is disposed.
[3] A flow-type reaction apparatus for continuously reacting two or more kinds of raw material substances, comprising: a mixing section for mixing two or more of the raw material substances; and a reaction section provided on a secondary side of the mixing section and obtaining a product by reacting the raw material substances, the mixing section including: a mixer for mixing two or more of the raw material substances; and two or more supply pipes for supplying the respective raw material substances to the mixer, the supply pipes being connected to the mixers, respectively, at least one of the supply pipes having a suppression mechanism at a connection portion of the supply pipe and the mixer, the suppression mechanism suppressing a movement of a fluid from the mixer toward the supply pipe, and at least one of the supply pipes being connected to the mixer from above with respect to a plane on which the mixer is provided.
[4] The flow reactor according to any one of [1] to [3], wherein the two or more raw material substances are a combination of one or more gaseous raw materials and one or more liquid raw materials.
[5] The flow-type reaction apparatus according to [2] or [3], wherein the two or more kinds of raw material substances are a combination of one or more kinds of gas raw materials and one or more kinds of liquid raw materials, at least one of the supply pipes for supplying the gas raw materials to the mixer is connected to the mixer from above with respect to a plane in which the mixer is provided, and at least one of the supply pipes for supplying the liquid raw materials to the mixer is connected to the mixer in parallel with the plane in which the mixer is provided.
[6] The flow-type reaction apparatus according to any one of [1] to [3], further comprising a separation unit that is provided on the secondary side of the reaction unit and separates a target substance from the product.
According to the flow reactor of the present invention, the reaction efficiency and the productivity sufficient for practical use can be maintained for a long time, and the size and the cost of the reaction equipment can be reduced.
Drawings
FIG. 1 is a system diagram schematically showing an example of the configuration of a flow reactor to which the first embodiment of the present invention is applied.
FIG. 2 is a cross-sectional view in the xy plane direction of a mixer provided in the flow reactor of the first embodiment.
FIG. 3 is a system diagram schematically showing an example of the structure of a flow-type reaction apparatus to which the second or third embodiment of the present invention is applied.
FIG. 4 is a cross-sectional view in the xz plane direction of a mixer provided in the flow reactor of the second embodiment.
FIG. 5 is a cross-sectional view in the xz plane direction of a mixer provided in a flow reactor according to a third embodiment.
Fig. 6 is a graph showing the change with time in the amount of gas raw material supplied in example 1.
FIG. 7 is a graph showing the change with time in the amount of gas raw material supplied in example 2.
FIG. 8 is a graph showing the change with time in the amount of gas raw material supplied in example 3.
Fig. 9 is a graph showing the change with time in the amount of gas raw material supplied in comparative example 1.
Detailed Description
The flow-type reaction apparatus according to the embodiment of the present invention will be described in detail below with reference to the drawings. In the drawings used in the following description, for the sake of easy understanding of the features of the present invention, the features may be enlarged for convenience, and the dimensional ratios of the components are not limited to be substantially the same.
< first embodiment >
First, the configuration of a flow reactor 1 according to a first embodiment to which an embodiment of the present invention is applied will be described.
Fig. 1 is a system diagram schematically showing an example of the structure of a flow reactor 1. In fig. 1, the vertical direction is the z-axis direction. As shown in fig. 1, the flow reactor 1 includes: a mixing section 10 for mixing two or more kinds of raw material substances; a reaction section 20 in which the raw material substances mixed by the mixing section 10 react in the reaction section 20; and a separation unit 30 for separating the target substance from the product produced by the reaction unit 20.
The respective components of the flow reactor 1 will be described in detail below.
The structure of the mixing section 10 is not particularly limited as long as two or more raw material substances can be mixed and a mixture containing each raw material substance can be supplied to the reaction section 20. The two or more kinds of raw material substances may be a combination of one or more kinds of gas raw materials and one or more kinds of liquid raw materials, a combination of two or more kinds of gas raw materials, or a combination of two or more kinds of liquid raw materials.
Next, the structure of the mixing section 10 will be described by taking as an example a case where two or more kinds of raw material substances are a combination of one or more kinds of gas raw materials and one or more kinds of liquid raw materials, and the target substance is diborane gas.
The mixing section 10 has: more than one gas raw material (BF)3Or BCl3Etc.) of a supply source 11; more than one liquid starting material (containing NaH or NaBH)4An ether solvent such as ethylene glycol dimethyl ether, diethylene glycol dimethyl ether, or triethylene glycol dimethyl ether) such as a reducing agent 12; a gas material supply path L11; a liquid material supply path L12; and a mixer (agitator) 13 connected to the two supply paths L11, L12.
The supply path L11 is provided with a pressure regulating valve 16 and a mass flow controller 17 from the primary side (upstream side). The supply path L12 is provided with a liquid feed pump 18 and a mass flow controller 19 from the primary side (upstream side).
The supply path L11 is a path for supplying the gas raw material to the mixer 13. The supply path 12 is a path for supplying the liquid material to the mixer 13.
The material of the pipes constituting the supply paths L11 and L12 is not particularly limited as long as it is not corroded by the gas material or the liquid material. The material of the pipe may be appropriately selected according to the properties of each raw material. Examples of the material of the pipe include a resin pipe such as Polytetrafluoroethylene (PTFE) and a metal pipe such as stainless steel (SUS).
The diameters of the pipes constituting the supply paths L11 and L12 are not particularly limited, and the diameters of the pipes may be appropriately selected according to the supply amounts of the raw material substances to be supplied to the mixer 13. For example, as the pipes constituting the supply paths L11 and L12, pipes having an outer diameter of 6 to 7mm and an inner diameter of 4 to 5mm can be used.
The mixer 13 is horizontally disposed on the xy plane shown in fig. 1. The mixer 13 is not particularly limited as long as it can mix the raw material substances (combination of the gas raw material and the liquid raw material) supplied through the two supply paths L11 and L12. As the mixer 13, a stirrer or the like can be exemplified.
The mixer 13 is connected to a supply path L21 provided in the reaction unit 20. Thereby, the mixing section 10 can supply the mixture of the respective raw material substances to the reaction section 20.
In the first embodiment, the supply path L11 is provided horizontally on the xy plane shown in fig. 1 with respect to the primary side portion L11A of the mixer 13 as a connecting portion with the mixer 13. Also, the supply path L12 is provided horizontally on the xy plane shown in fig. 1 with respect to the primary side portion L12A of the mixer 13 as a connecting portion with the mixer 13. That is, in the first embodiment, the primary-side parts L11A, L12A as the connection parts with the mixer 13 in the supply paths L11, L12 are horizontally arranged on the same plane as the mixer 13.
FIG. 2 is a cross-sectional view showing the mixer 13 provided in the flow reactor 1 in the xy plane direction.
The white arrows shown in fig. 2 indicate the directions of the respective raw material substances flowing in the respective supply paths L11, L12 and the raw material substance mixture flowing in the supply path L21.
As shown in fig. 2, in the first embodiment, the supply path L11 has the orifice S near the connection portion of the supply path L11 and the mixer 13.
The orifice S is for narrowing at least a part of the gas raw material flow passage (raw material substance flow passage) in the pipe configuring the supply path L11. Since the orifice S is provided in the vicinity of the connection portion of the supply path L11A with the mixer 13, a part of the gas material flow path is narrowed, and the fluid such as liquid can be prevented from flowing back from the mixer 13 to the supply path L11. As described above, the orifice S is an example of a suppressing mechanism for suppressing the fluid in the mixer 13 from moving from the mixer 13 to the supply flow path L11.
The shape of the orifice S is not particularly limited as long as it is a shape capable of preventing the liquid in the mixer 13 from flowing backward. The orifice S can be appropriately selected according to the properties of the raw material and the internal structure of the pipe constituting the supply path L11. Examples of the orifice S include a hole and a T-joint having a different diameter.
In fig. 2, S1 denotes an inner diameter of a pipe configuring the supply path L21, and S2 denotes a flow passage diameter of a portion where the flow passage is locally narrowed by the throttle S.
In the first embodiment, the throttle ratio (S2/S1) is preferably about 0.1 to 0.75. If the throttle ratio is equal to or higher than the lower limit, the supply pressure of the gas raw material can be stabilized easily, and the raw materials can be continuously supplied to the mixer 13 easily. If the throttle ratio is equal to or less than the upper limit value, the liquid backflow caused by the pressure fluctuation in the reaction unit 20 can be easily suppressed, and the pipe constituting the supply path L11 can be easily prevented from being clogged.
In fig. 2, S3 denotes the length of the throttle piece S in the supply direction of the gas raw material. In the first embodiment, the length S3 of the orifice is preferably about 0.1 to 10 mm. If the length S3 of the throttle is equal to or greater than the lower limit value, the physical strength of the throttle S is easily maintained, and the throttle S is less likely to be damaged. If the length S3 of the orifice is equal to or less than the upper limit value, the pipe configuring the supply path L11 is less likely to be clogged, and the reaction efficiency is easily maintained for a long time.
In fig. 2, S4 indicates the length of the supply path L11 after the throttle is opened. In the first embodiment, the post-throttle-opening length S4 on the gas pipe side is preferably 0 to 10 mm. When the length S4 is within the above range, the synthesis yield is less likely to decrease. The length S4 of the supply path L11A after the throttle is opened is more preferably 0 mm.
That is, the phrase "the supply path L11 has the orifice S near the connection portion between the supply path L11 and the mixer 13" means that the supply path L11 has the orifice S at the connection portion between the supply path L11 and the mixer 13 so that the length S4 of the supply path L11A after the orifice is opened is 0 to 10 mm.
The parameters of S1, S2, S3 and S4 described above can be appropriately selected according to the chemical reaction system to which the flow reactor 1 is applied. That is, each of the above parameters can be appropriately selected depending on a combination of two or more kinds of raw material substances or the like.
The mixing section 10 having the above configuration can continuously supply a mixture including a gas raw material and a liquid raw material to the reaction section 20 by continuously supplying the gas raw material and the liquid raw material to the mixer 13 and mixing them by the mixer 13. As described above, the mixing section 10 is an example of one embodiment of a device for mixing two or more kinds of material substances that are continuously supplied.
Temperature adjusting mechanisms such as heaters may be provided in the supply paths L11 and L12. This makes it possible to adjust the temperature of the supply paths L11 and L12 to a temperature suitable for the chemical reaction of the raw material substances.
The reaction part 20 is provided at the secondary side of the mixing part 10. The reaction unit 20 includes a supply path L21 of the raw material mixture mixed by the mixing unit 10, a reaction field 21 provided on the supply path L21, and a back pressure valve 22 provided on the supply path L21 between the reaction field 21 and the separation unit 30.
The supply path L21 is a path connecting the mixing section 10 and the separation section 30. A first end of a pipe configuring the supply path L21 is connected to the mixer 13, and a second end is connected to the separation section 30. Thereby, the reaction portion 20 can supply the fluid flowing through the supply path L21 to the separation portion 30.
The material of the pipe constituting the supply passage L21 is not particularly limited, and the same material as that of the supply passages L11 and L12 can be used.
The diameter of the pipe configuring the supply path L21 may be appropriately selected according to the supply amount of the mixture supplied to the separation section 30. Specifically, for example, a pipe having an outer diameter of 1 to 30mm can be used.
The reaction field 21 is a field in which two or more kinds of raw material substances (gas raw material and liquid raw material) are chemically reacted. The reaction field 21 is not particularly limited as long as it is in a form that can control the reaction time of the chemical reaction. For example, in the present embodiment, the reaction field 21 is constructed of a spiral pipe.
The length of the pipe configuring the reaction field 21 may be appropriately selected according to various factors such as the raw material substance, the target substance, or the reaction efficiency of the chemical reaction. For example, when the reaction time is set to a long time, the length of the pipe of the reaction field 21 may be increased. When the reaction time is set to a short time or when a chemically unstable reaction intermediate is prepared as a target substance, the length of the pipe of the reaction field 21 may be shortened. The material of the pipe constituting the reaction field 21 can be appropriately selected depending on various factors such as the temperature and pressure at the time of the chemical reaction.
The inner diameter of the pipe constituting the reaction field 21 is preferably 2mm or more. If the inner diameter is equal to or greater than the lower limit value, clogging in the reaction field 21 can be easily prevented, so that the supply amount of the raw material can be sufficiently maintained, and high productivity can be easily achieved.
The inner diameter of the pipe constituting the reaction field 21 is preferably 30mm or less. If the inner diameter is not more than the upper limit, the reaction efficiency of the chemical reaction in the reaction field 21 is easily improved.
The back pressure valve 22 is a valve that controls the pressure of the reaction field 21. This makes it possible to maintain the pressure of the reaction field 21 at a pressure suitable for the chemical reaction of the raw material substance, and to supply the product generated in the reaction field 21 to the separation unit 30 at a stable flow rate. Further, by providing the back pressure valve 22 on the primary side (upstream side) of the separator 30, the product can be continuously supplied to the gas-liquid separator 31 while maintaining the reduced pressure state of the gas-liquid separator 31 provided in the separator 30.
According to the reaction section 20 having the above configuration, the product can be obtained by continuously chemically reacting the raw material substances mixed by the mixing section 10. The reaction unit 20 can continuously supply a product (a mixture containing diborane gas and a solvent in a gas-liquid coexisting state) generated by the chemical reaction to the separation unit 30. Thus, the reaction section 20 is an example of a device for controlling the continuous chemical reaction of the raw material substance.
The separation part 30 is provided at the secondary side of the reaction part 20. The separation section 30 has: a gas-liquid separator 31 connected to the supply path L21; a gas recovery path L31 for discharging the gas in the gas-liquid separator 31 to the outside of the gas-liquid separator 31; a liquid recovery path L32 for discharging the liquid in the gas-liquid separator 31 to the outside of the gas-liquid separator 31; and a control device 32.
The gas-liquid separator 31 is a container that separates a mixture containing gas and liquid in a gas-liquid coexisting state into gas and liquid and stores the gas and liquid in an airtight space provided inside.
The inner space of the gas-liquid separator 31 communicates with the supply path L21. Thereby, the mixture is supplied into the gas-liquid separator 31 through the supply path L21. Further, the airtight space inside the gas-liquid separator 31 is divided into a gas phase 31A and a liquid phase 31B.
The gas-liquid separator 31 may be a metal container such as stainless steel. The gas-liquid separator 31 is preferably capable of withstanding a reduced pressure state (for example, 20 to 40kPa abs.).
The volume, inner diameter and height of the gas-liquid separator 31 can be appropriately selected depending on factors such as the yield of the target substance and the size of the flow reactor 1.
In the present embodiment, the inner diameter of the gas-liquid separator 31 is preferably 50 to 200 mm. If the inner diameter is not less than the lower limit, the gas-liquid separation is sufficiently performed, and the yield of the target substance is easily improved. Further, if the inner diameter is not more than the upper limit, the flow reactor 1 can be easily downsized.
In the present embodiment, the height of the gas-liquid separator 31 is preferably 200 to 800 mm. If the height is not less than the lower limit, the gas-liquid separation is sufficiently performed, and the yield of the target substance is easily improved. Further, if the height is not more than the upper limit, the flow reactor 1 can be easily downsized.
Here, the gas-liquid separator 31 is not particularly limited to the container form as long as it can separate a mixture containing gas and liquid in a gas-liquid coexisting state into gas and liquid and store the gas and liquid in the airtight space provided inside. For example, the following structure is also possible: that is, the airtight space is provided by setting the diameter of a part of the pipe connecting between the supply path L21 and the liquid recovery path L32 to be at least larger than the diameter of the supply path L21. According to this structure, the mixture containing the gas and the liquid in the gas-liquid coexisting state can be separated into the gas and the liquid, and stored in the airtight space provided inside, respectively.
The gas-liquid separator 31 is provided with a liquid level gauge 33. The liquid level gauge 33 can detect the height of the interface (i.e., the liquid level) between the gas phase 31A and the liquid phase 31B in the space inside the gas-liquid separator 31. Here, the liquid level meter 33 is not particularly limited as long as it can detect the height of the liquid level in the gas-liquid separator 31. The liquid level gauge 33 may be a float type, reflection type, tube type, or see-through type.
The gas recovery path L31 is a pipe communicating with the gas phase 31A of the gas-liquid separator 31. Further, the gas recovery path L31 is provided with an opening degree adjustment valve 34 and a pressure reducer 35 in this order from the primary side (upstream side).
The opening degree adjustment valve 34 is a valve that adjusts the opening degree of the duct constituting the gas recovery path L31. This enables adjustment of the flow rate of the gas flowing through the gas recovery passage L31. The opening adjustment valve 34 is not particularly limited, and an automatic needle valve, a butterfly valve, or the like can be exemplified.
The pressure reducing device 35 is a device for reducing the pressure in the gas recovery path L31. The pressure reducing device 35 is not particularly limited, and a pressure reducing pump and the like can be exemplified. The pressure reducing device 35 is provided in the gas recovery path L31 to suck and recover the target substance (diborane gas) from the gas phase 31A in the gas-liquid separator 31.
The capacity of the pressure reducing device 35 is not particularly limited as long as it is a form capable of reducing the pressure of the gas phase 31A of the gas-liquid separator 31 to a predetermined pressure (for example, about 50 to 500hPa abs.). The pressure reducing device 35 may be appropriately selected according to the composition of the mixture supplied into the gas-liquid separator 31. The pressure reducing device 35 may be exemplified by a vacuum pressure reducing pump (for example, manufactured by Povid corporation (イワキ Co., Ltd.), "BA-106F", or the like).
According to the flow reactor 1, the pressure of the gas phase 31A of the gas-liquid separator 31 can be reduced to a constant pressure of, for example, about 50 to 500hPa abs. Then, the target substance (diborane gas) can be recovered from the secondary side of the pressure reducing device 35.
In this way, the gas recovery path L31 can discharge the target substance and the like in the gas phase 31A continuously supplied to the gas-liquid separator 31 from the gas-liquid separator 31 while adjusting the flow rate.
The material of the duct constituting the gas recovery passage L31 is not particularly limited, and the same materials as those of the supply passages L11, L12, and L21 can be used. The diameter of the pipe configuring the gas recovery passage L31 is not particularly limited, and pipes having the same diameter as the supply passages L11, L12, and L21 can be used.
As necessary, a flow meter for measuring the yield of the target substance (diborane gas) to be recovered, a container for storing the target substance, a purifier for purifying the target substance, or an analyzer (for example, FT-IR) for analyzing the concentration of the target substance may be provided on the secondary side of the pressure reducing device 35 in the gas recovery path L31 as appropriate. The gas recovery path L31 may be connected to a subsequent reaction device or the like on the secondary side of the pressure reducing device 35.
The liquid recovery path L32 is a conduit communicating with the liquid phase 31B of the gas-liquid separator 31. An on-off valve (opening/closing device) 36 is provided in the liquid recovery path L32.
The opening/closing valve 36 is not particularly limited as long as it switches the opening/closing of the pipe configuring the liquid recovery path L32. The opening/closing valve 36 may be, for example, a manual diaphragm valve or a ball valve.
By opening the opening/closing valve 36, the discharge of the liquid from the gas-liquid separator 31 into the gas-liquid recovery path L32 can be started. On the other hand, by closing the opening/closing valve 36, the discharge of the liquid from the gas-liquid separator 31 to the gas-liquid recovery path L32 can be stopped. Thereby, the liquid recovery path L32 can discharge the liquid continuously supplied to the gas-liquid separator 31.
The material of the pipe constituting the liquid recovery path L32 is not particularly limited, and the same material as the supply paths L11, L12, and L21 or the gas recovery path L31 can be used. Further, the diameter of the pipe configuring the liquid recovery path L32 is not particularly limited, and a pipe having the same diameter as the supply paths L11, L12, and L21 or the gas recovery path L31 can be used.
Note that a refining device capable of condensing the solvent such as an evaporator may be provided on the secondary side of the opening/closing valve 36 of the liquid recovery path L32. Thereby, the ether solvent discharged from the gas-liquid separator 31 is introduced into the refining apparatus. Thereby, the ether solvent condensed and purified can be reused as a liquid raw material. The solid mixed into the above solvent is separated from the solvent and discarded as a solid.
In the refining apparatus, diborane gas dissolved in the ether solvent is separated and recovered from the liquid. This enables the target substance (diborane gas) to be recovered with higher efficiency.
The control device 32 includes, as an operation control system, a controller for driving each driving unit and a control unit for controlling each controller. Each controller is formed of, for example, a proportional-integral-derivative (PID) controller or the like, and is electrically connected to actuators and the like provided in the liquid level gauge 33, the opening-degree regulating valve 34, the opening/closing valve 36, and the like, and performs start, stop, adjustment, and the like of each portion. Thus, the respective controllers can control the conditions such as the pressure and the liquid surface height in the gas-liquid separator 31 to be constant.
According to the separation unit 30 having the above-described structure, diborane gas as a target substance can be separated from the product (a mixture containing diborane gas and a solvent in a gas-liquid coexisting state) produced in the reaction unit 20. As described above, the separation unit 30 is an example of an apparatus that separates and separately collects at least gas and liquid from a mixture containing the gas and the liquid in a gas-liquid coexisting state.
Next, an example of the operation method of the flow reactor 1 will be described.
First, in the mixing section 10, the flow rate is adjusted by the mass flow controller 19 from the liquid raw material supply source 12 through the supply path L12, and the ether solvent is continuously supplied to the mixer 13 by the liquid feed pump 18.
Subsequently, BF is adjusted by the pressure regulating valve 16 from the gas raw material supply source 11 via the supply path L113Or BCl3The pressure of the boron trihalide gas is equalized, and the flow rate of the boron trihalide gas is adjusted by the mass flow controller 17, and the boron trihalide gas is supplied to the mixer 13.
Here, the supply conditions of the liquid raw material are not particularly limited, and may be appropriately selected depending on various factors. For example, when the liquid raw material is supplied, the pressure is 0.1 to 1.5MPaG, the flow rate is 50 to 2000 mL/min, and the concentration is 0.25 to 2 mol/L. Similarly, the supply conditions of the gas raw material are not particularly limited, and may be appropriately selected depending on various factors. For example, when the gas raw material is supplied, the pressure is 0.1 to 1.5MPaG, the flow rate is 1.5 to 3L/min, and the concentration is 100 mol%.
The gas raw material and the liquid raw material are mixed in the mixer 13. The form of mixing the gaseous raw material and the liquid raw material is not particularly limited. For example, the gas material and the liquid material may be alternately and continuously supplied, and the gas material and the liquid material may be mixed by forming plug flows in which the gas material and the liquid material are alternately divided into small pieces. Thereby, the gas raw material and the liquid raw material can be mixed immediately, and high mixing uniformity can be achieved.
In the reaction section 20, the mixed gas raw material and liquid raw material continuously react. Thereby, a product containing diborane gas as a target substance and an ether solvent in a gas-liquid coexisting state is continuously produced. The reaction by-product may be contained in the product.
The product is continuously supplied into the gas-liquid separator 31 at a constant flow rate through the back pressure valve 22 provided in the supply passage L21. During this period, the gas-liquid separator 31 maintains the pressure-reduced state by the back pressure valve 22.
Here, the reaction conditions of the reaction section 20 are not particularly limited, and the reaction conditions of the reaction section 20 may be appropriately selected depending on various factors. For example, when the above-mentioned product is produced, the conditions that the residence time in the reaction field 21 is 1 second to 10 minutes and the pressure in the reaction field 21 is 0.01 to 1MPaG can be applied.
The product supplied into the gas-liquid separator 31 is separated into diborane gas and the ether solvent, and a gas phase 31A and a liquid phase 31B are formed in the gas-liquid separator 31, respectively. The inside of the gas-liquid separator 31 is depressurized by a depressurizing device 35 provided in a gas recovery path L31 communicating with the gas phase 31A.
The pressure-reduced state in the gas-liquid separator 31 is controlled to be kept constant by the control device 32. The conditions such as the pressure and the liquid surface height in the gas-liquid separator 31 are not particularly limited, and the conditions such as the pressure and the liquid surface height in the gas-liquid separator 31 may be appropriately selected depending on various factors. For example, the pressure in the gas-liquid separator 31 may be set to 20 to 40kPa abs, and the liquid level in the gas-liquid separator 31 may be set to 70 to 100mm from the bottom of the gas-liquid separator 31.
Here, diborane gas in the gas-liquid separator 31 is recovered from the secondary side of the pressure reducing device 35.
The recovered diborane gas may be recovered after being refined by a refiner provided at a subsequent stage, or may be supplied to a reaction apparatus or the like provided at a subsequent stage.
If the product is continuously supplied into the gas-liquid separator 31 and diborane gas is recovered, the liquid phase 31B in the gas-liquid separator 31 increases and the liquid level rises. If the position of the liquid level reaches a predetermined set value inputted to the liquid level gauge 33, the signal value is transmitted to the control device 32.
Then, an open signal is sent from the control device 32 to the on-off valve 36. The on-off valve 36 receiving the signal is opened, and the ether solvent in the gas separator 31 is discharged to the liquid recovery path L32. Thereby, the ether solvent containing the by-product is recovered. The discharged ether solvent and by-products may be recovered after refining in a refining unit provided at a subsequent stage, or may be supplied to the supply source 12 of the liquid raw material and reused.
If the ether solvent is recovered, the liquid phase 31B in the gas-liquid separator 31 decreases and the liquid level falls. If the liquid surface position reaches a predetermined set value input to the liquid level gauge 33, the signal value is transmitted to the control device 32, and the control device 32 transmits a closing signal to the opening/closing valve 36. The on-off valve receiving the signal is in the closed state, and the discharge of the ether solvent in the gas-liquid separator 31 to the liquid recovery path L32 is stopped.
As described above, the flow reactor 1 can continuously produce diborane gas, which is a target substance, by continuously supplying gaseous raw materials and liquid raw materials and continuously reacting these raw materials. In the present embodiment, the flow reaction apparatus 1 was described by taking the production of diborane gas as an example, but the present embodiment may be applied to the production of other chemical substances.
For example, the flow reactor 1 may use an acid such as acetic acid or hydrochloric acid, NaH or NaBH as the raw material4Etc. to prepare the hydrogen structure. In addition, the structure may be such that carbon dioxide is produced using calcium carbonate and hydrochloric acid as raw materials. Alternatively, the chlorine gas may be produced using perchloric acid and hydrochloric acid as raw materials. The compounds exemplified herein are examples, and the application of the flow reactor 1 is not limited to these examples.
According to the flow reactor 1 of the first embodiment described above, even if the pressure of the reaction field 21 suddenly fluctuates due to the chemical reaction and the liquid flows back in the mixer, the liquid can be pushed back by the throttle S. Therefore, the flow reactor 1 is less likely to cause backflow of the liquid in the mixer, and can prevent clogging of the supply path due to the backflow. Therefore, the flow reactor 1 can continuously supply the gas raw material to the mixer, and therefore, even when the apparatus is operated for a long time, it is difficult to reduce the reaction efficiency, and high productivity can be maintained.
In addition, the flow reactor 1 can prevent the clogging of the piping by providing the orifice S in the supply path L11. Since the throttle body S does not need a complicated structure such as an ultrasonic transducer, the size and cost of the device can be reduced.
The flow reaction apparatus 1 of the first embodiment can be suitably applied to the following chemical reaction system: in this chemical reaction system, even when the supplied raw material substance is retained in the mixer 13, the reaction efficiency of the chemical reaction and the like are less affected.
(modification of the first embodiment)
Next, a flow-type reaction apparatus according to modification 1 of the first embodiment will be described. Modification 1 of the first embodiment is different from flow reactor 1 in that it has the same configuration as flow reactor 1 except that a throttle S is provided in supply path L12A near the connection portion between supply path L12 and mixer 13, and no throttle S is provided in supply path L11 near the connection portion between supply path L11 and mixer 13.
The flow reactor of modification 1 of the first embodiment can also obtain the same operational advantages as the flow reactor 1.
(modification 2 of the first embodiment)
Next, a flow-type reaction apparatus according to modification 2 of the first embodiment will be described. Modification 2 of the first embodiment is different from flow reactor 1 in that a configuration similar to that of flow reactor 1 is provided except that a throttle S is provided in two portions, namely, supply path L11A near the connection portion between supply path L11 and mixer 13 and supply path L12A near the connection portion between supply path L12 and mixer 13.
The flow reactor of modification 2 of the first embodiment can also obtain the same operational advantages as the flow reactor 1.
< second embodiment >
Next, the structure of the flow reactor 2 according to the second embodiment of the present invention will be described.
Fig. 3 is a system diagram schematically showing an example of the structure of the flow reactor 2. In fig. 3, the z-axis direction is the vertical direction as in fig. 1. As shown in fig. 3, the flow reactor 2 of the second embodiment includes a mixer 14 instead of the mixer 13. In addition, in the second embodiment, a portion L11 as a connecting portion with the mixer 14 in the supply path L11 with respect to the primary side of the mixer 14 is connected to the mixer 14 from above with respect to the xy plane shown in fig. 3.
The flow reactor 2 of the second embodiment is different from the flow reactor 1 in the structure described above, and has the same structure as the flow reactor 1 except that it is different from the flow reactor 1. Hereinafter, the explanation of the same components as those of the flow reactor 1 will be omitted.
FIG. 4 is a cross-sectional view in the xz plane direction of the mixer 14 provided in the flow reactor 2. As shown in fig. 4, in the second embodiment, a portion L11A on the primary side of the mixer 14, which is a connection portion with the mixer 14 in the supply path L11, is connected to the mixer 14 from above the xy plane in the z-axis direction, i.e., from vertically above. In the second embodiment, no orifice is provided in each of the supply paths in the vicinity of the connection portion between the mixer 14 and the supply path L11 and in the vicinity of the connection portion between the mixer 14 and the supply path L12.
In the second embodiment, the gas raw material is introduced from above the mixer 14 (in the z-axis direction) through the supply path L11. Thus, even if the liquid attempts to flow back toward the supply path L11, the liquid can be pushed back from above by the supply gas material. Even if the liquid in the mixer 14 attempts to flow back toward the supply path L11, the liquid is unlikely to flow back because of gravity acting on the gas material being supplied.
According to the flow reactor 2 of the second embodiment described above, the liquid in the mixer 14 is unlikely to flow backward, and even if the liquid flows backward, the liquid is likely to be quickly led out from the pipe constituting the supply path L11 by the action of gravity, and is unlikely to stay in the pipe for a long time. This makes it difficult to dry the liquid and cause clogging due to precipitation of solids. Therefore, the flow reactor 2 exhibits the same operational advantages as the flow reactor 1 of the first embodiment.
The flow reactor 2 of the second embodiment can be suitably used in a chemical reaction system in which a difference in compressibility between two or more types of raw material substances is small at the time of chemical reaction, a chemical reaction system in which pressure fluctuation due to chemical reaction is small, or the like.
(modification of the second embodiment)
Next, a flow reactor according to a modification of the second embodiment will be described. The modification of the second embodiment is different from the flow reactor 2 in that the flow reactor 2 has the same configuration as the flow reactor 2 except that a portion L11A on the primary side of the mixer 14, which is a connection portion with the mixer 14 in the supply path L11, forms an angle of ω ° with respect to the z-axis and is connected to the mixer 14 from above with respect to the xy-plane.
The above ω is preferably set in the range of 0 to 45 °. If ω is equal to or less than the upper limit value, even if the liquid in the mixer 14 flows backward, the liquid can be easily and quickly led out from the pipe configuring the supply path L11.
The flow reactor according to the modification of the second embodiment can also obtain the same operational advantages as the flow reactor 2.
< third embodiment >
Next, the structure of the flow reactor 3 according to the third embodiment of the present invention will be described.
Fig. 3 is a system diagram schematically showing an example of the structure of the flow reactor 3. As shown in fig. 3, the flow reactor 3 of the third embodiment includes a mixer 15 instead of the mixers 13 and 14. In addition, in the third embodiment, a portion L11A with respect to the primary side of the mixer 15, which is a connecting portion with the mixer 15 in the supply path L11, is connected to the mixer 15 from above with respect to the xy plane shown in fig. 3.
The flow reactor 3 of the third embodiment is different from the flow reactor 1 in the structure described above, and has the same structure as the flow reactor 1 except that it is different from the flow reactor 1. Hereinafter, the same structural parts as those of the flow reactor 1 will not be described.
FIG. 5 is a cross-sectional view in the xz plane direction of the mixer 15 provided in the flow reactor 3. As shown in fig. 5, in the third embodiment, a throttle S is provided on the supply path L11A in the vicinity of the connection portion of the supply path L11 and the mixer 15.
In fig. 5, S4 indicates the length of the supply path L11A (L11) after the throttle is opened. In the third embodiment, the post-throttle-opening length S4 on the gas pipe side is preferably 0 to 10 mm. If the length S4 is within the above range, it is difficult to cause a decrease in the synthesis yield. The length S4 of the supply path L11A after the throttle is opened is more preferably 0 mm.
That is, "the throttle S is provided in the supply path L11A near the connection portion between the supply path L11 and the mixer 15" means that the supply path L11A has the throttle S at the connection portion between the supply path L11A and the mixer 15 so that the length S4 of the supply path L11A (L11) after the throttle is opened is 0 to 10 mm.
Since the orifice S is provided in the supply path L11A near the connection portion with the mixer 15, the liquid can be prevented from flowing backward from the mixer 15 toward the supply path L11. The detailed configurations of the shape, type, throttle ratio (S2/S1), throttle length S3, post-throttle-opening length S4, and the like of the throttle S may be the same as those described in the first embodiment.
As shown in fig. 5, in the third embodiment, a portion L11 on the primary side of a portion of the supply path L11 connected to the mixer 15 is connected to the mixer 15 from above with respect to the xy plane in the z-axis direction, i.e., from vertically above. Thus, even if the liquid flows backward through the supply path L11, the backward flow of the liquid can be pushed back from above by the supply of the gas material. Even if the liquid in the mixer 15 flows back toward the supply path L11, the liquid flowing back is quickly led out from the supply path L11 by the action of gravity.
According to the flow reactor 3 of the third embodiment described above, productivity and reaction efficiency sufficient for practical use can be maintained for a longer period of time, in addition to the same operational effects as those of the flow reactor 1 of the first embodiment. Further, since the flow reactor 3 enhances the backflow prevention effect and the retention suppression effect in the mixer as compared with the flow reactors 1 and 2, the target substance can be continuously produced even in the case of a high-pressure target substance (diborane gas) of about IMPaG, and in addition, it is difficult to cause drying of the liquid and clogging due to precipitation of the solid, and the operation and stop of the flow reactor can be repeated arbitrarily regardless of the number of times.
(modification 1 of the third embodiment)
Next, a flow-type reaction apparatus according to modification 1 of the third embodiment will be described. Modification 1 of the third embodiment is different from the flow reactor 3 in that it has the same configuration as the flow reactor 3 described above except that the orifice S is provided in the supply path L12A near the connection portion between the supply path L12 and the mixer 15, and the orifice S is not provided in the supply path L11A near the connection portion between the supply path L11 and the mixer 15.
The flow reactor of modification 1 of the third embodiment can also obtain the same operational advantages as the flow reactor 3.
(modification 2 of the third embodiment)
Next, a flow-type reaction apparatus according to modification 2 of the third embodiment will be described. Modification 2 of the third embodiment is different from the flow reactor 3 in that the same configuration as that of the flow reactor 3 is provided except that the throttle body S is provided in two portions, namely, the supply path L11A near the connection portion between the supply path L11 and the mixer 15 and the supply path L12A near the connection portion between the supply path L12 and the mixer 15.
The flow reactor of modification 2 of the third embodiment can also obtain the same operational advantages as the flow reactor 3.
< other embodiment >
Next, the structure of a flow reactor according to another embodiment of the present invention will be described.
The flow reactor of the present embodiment has the same configuration as the flow reactor 1 except that the separation unit 30 includes the pressure reducing device 35 and further includes a second pressure reducing device.
The second pressure reducing device is provided in the liquid recovery path L32. Thereby, the second pressure reducing device can reduce the pressure in the liquid recovery path L32. In addition, the second pressure reducing device is electrically connected to the control device 32.
The capacity of the second depressurizing device is not particularly limited as long as it can depressurize to the same or higher pressure as the pressure in the gas-liquid separator 31 (the pressure of the gas phase 31A), and the capacity of the second depressurizing device can be appropriately selected according to the capacity of the depressurizing device 35. Additionally, the second pressure relief device may be the same as or different from the pressure relief device 35.
In the present embodiment, if the position of the liquid surface of the liquid phase 31B in the gas-liquid separator 31 reaches the predetermined set value input to the liquid surface gauge 33, the signal value is transmitted to the control device 32, and the control device 32 outputs the operation signal to the second depressurizing device. Thus, the second depressurizing device starts operating under the condition that the pressure in the liquid recovery path L32 is lower than the pressure in the gas-liquid separator 31.
According to the flow reactor of the other embodiment described above, the liquid recovery path L32 can be set to a pressure lower than the pressure in the gas-liquid separator 31. Therefore, according to the present embodiment, it is possible to easily collect the liquid from the liquid phase 31B in the gas-liquid separator 31 through the liquid collection path L32, and it is possible to make it difficult for air to be mixed into the gas-liquid separator 31 in a depressurized state.
While several embodiments of the present invention have been described above, the present invention is not limited to the specific embodiments described above. The present invention may be modified in addition to or in addition to the above-described embodiments within the scope of the present invention as defined in the appended claims.
For example, in the embodiment described above, the primary-side portion L12A of the portion of the supply path L12 for the liquid material connected to the mixer is arranged on the xy plane and connected to the mixer, but the portion L12 may be connected to the mixer from above the xy plane.
Further, the following structure may be adopted: that is, without using a mixer such as a stirrer, the secondary side end of the supply path L11 and the secondary side end of the supply path L12 are connected, and instead of the mixer, a junction portion where the supply path L11 and the supply path L12 join is used, and two or more raw material substances are mixed at the junction portion.
< example >
The present invention will be specifically described below with reference to examples, but the present invention is not limited to the following descriptions.
(example 1)
The flow type reaction apparatus 1 of the first embodiment was used to continuously synthesize diborane gas. As specific reaction conditions, BF was used3As the gaseous raw material, an ether solvent in which a reducing agent is dissolved in ether is used as the liquid raw material. The throttle ratio of the throttle S (S2/S1) was set to 0.25, the length of the throttle S3 was set to 1mm, and the post-throttle-opening length was set to 0 mm.
The liquid raw material used is distilled and purified by an evaporator (not shown) provided on the secondary side (downstream side) of L32, and the liquid raw material is reintroduced into the liquid raw material supply source 12 and circulated for reuse. The flow rate of the diborane gas recovered from the gas recovery path L31 is measured by a float flowmeter (not shown) provided on the secondary side of the pressure reducing device 35. The purity of the produced diborane gas was measured by an infrared spectrometer (FT-IR, not shown) provided on the secondary side of the pressure reducing device 35.
Fig. 6 is a graph showing the change with time in the supply amount of the gas raw material in example 1. As shown in FIG. 6, in example 1, BF was continuously supplied for 35 minutes or more3Gas, and can continuously synthesize diborane gas. In addition, the yield of diborane gas is about 85-90% as a result of measurement by using a flow meter. As a result of analyzing the obtained diborane gas by FT-IR, the purity of the diborane gas was 99 mol%.
In example 1, BF was started3After 40 minutes of gas supply, BF supply was stopped3After the synthesis reaction is stopped, the synthesis reaction is started again. As a result, as shown by the peak around 50 minutes on the horizontal axis in FIG. 1, the line of the supply path was blocked during the stop of the synthesis reaction in the flow reactor of example 1, and BF could not be supplied even when the synthesis reaction was to be restarted3A gas.
(example 2)
Diborane gas was synthesized under the same conditions as in example 1, except that the flow reactor 2 of the second embodiment was used.
FIG. 7 is a graph showing the change with time in the amount of gas raw material supplied in example 2. As shown in FIG. 7, in example 2, BF was continuously supplied for about 20 minutes3Gas, and can continuously synthesize diborane gas. However, then BF3The supply amount of the gas rapidly decreases, suggesting clogging of the pipe of the supply path, and the like. In addition, the yield of diborane gas is about 85-90% as a result of measurement by using a flow meter. As a result of analyzing the obtained diborane gas by FT-IR, the purity of the diborane gas was 99 mol%.
(example 3)
Diborane gas was synthesized under the same conditions as in example 1, except that the flow reactor 3 of the third embodiment was used.
FIG. 8 shows an embodiment3, the change with time in the supply amount of the gas raw material. As shown in FIG. 8, in example 3, BF was continuously supplied for 160 minutes or more3Gas, and can continuously synthesize diborane gas. In addition, the yield of diborane gas is about 85-90% as a result of measurement by using a flow meter. As a result of analyzing the obtained diborane gas by FT-IR, the purity of the diborane gas was 99%. As a result of FT-IR analysis of the solvent recovered from the evaporator, BF as a gaseous raw material was not observed3And (4) gas residue.
In example 3 as well, the synthesis reaction was stopped and then restarted as in example 1. As a result, during the stop of the synthesis reaction, there was no sign indicating clogging of the pipe of the supply path, and BF could be supplied smoothly as before the stop of the synthesis reaction3A gas.
Comparative example 1
Diborane gas was synthesized in the same manner as in example 1 except that the mixer 13 was replaced with a mixer having no throttle element, and the primary side portion L11A of the connection portion of the supply path L11 with the mixer was horizontally disposed on the xy plane, instead of vertically above the mixer, in the flow reactor shown in fig. 1.
Fig. 9 is a graph showing the change with time in the supply amount of the gas raw material in comparative example 1. As shown in fig. 9, in the comparative example, the supply amount of the gas raw material was unstable after 15 minutes from the start of the operation, and the gas raw material could hardly be supplied after 20 minutes from the start of the operation. The deposition of the solvent and the solid was observed when the inside of the supply path L11 was visually checked, which suggests that the pipe was clogged due to the reverse flow. During the period from the start of operation to 15 minutes or less, the purity and yield of diborane gas were not found to be greatly different from those of the examples, but after 15 minutes had elapsed, the yield of diborane gas was greatly reduced, and the purity of diborane gas was also reduced.
The results of the above examples and comparative examples show that the flow-type reaction apparatus of examples 1 to 3 can be operated continuously for a long period of time. The flow reactor of example 3 is shown to be capable of repeating the stop and restart of the synthesis reaction.
It is to be noted that the yield of diborane gas obtained in each example was at a level sufficient for practical use. In addition, the purity of the diborane gas is higher, and high-quality diborane gas can be obtained.
Description of the reference numerals
1. 2, 3 flow type reaction device
10 mixing section
11 supply source of gas raw material
12 supply source of liquid raw material
13. 14, 15 mixer
16 pressure regulating valve
17 mass flow controller
18 liquid feeding pump
19 mass flow controller
20 reaction part
21 reaction field
22 back pressure valve
30 separating part
31 gas-liquid separator
31A gas phase
31B liquid phase
32 control device
33 liquid level gauge
34 degree regulating valve
35 pressure reducing device
36 opening and closing valve
L11, L12, L21 supply paths
L31 gas recovery route
L32 liquid recovery route
S throttling element
S1 inner diameter
S2 flow passage diameter
Length of S3 throttle
S4 Length of supply Path after opening throttle

Claims (6)

1. A flow-type reaction apparatus for continuously reacting two or more kinds of raw material substances, comprising:
a mixing section for mixing two or more of the raw material substances; and
a reaction section provided on the secondary side of the mixing section and obtaining a product by reacting the raw material substances,
the mixing section has: a mixer for mixing two or more of the raw material substances; and two or more supply lines for supplying the respective raw material substances to the mixer,
the supply pipes are connected to the mixers, respectively, and at least one of the supply pipes has a suppression mechanism in the vicinity of a connection portion of the supply pipe and the mixer, the suppression mechanism suppressing movement of the fluid from the mixer to the supply pipe.
2. A flow-type reaction apparatus for continuously reacting two or more kinds of raw material substances, comprising:
a mixing section for mixing two or more of the raw material substances; and
a reaction section provided on the secondary side of the mixing section and obtaining a product by reacting the raw material substances,
the mixing section has: a mixer for mixing two or more of the raw material substances; and two or more supply lines for supplying the respective raw material substances to the mixer,
the supply lines are connected to the mixers, respectively, and at least one of the supply lines is connected to the mixer from above with respect to a plane in which the mixer is disposed.
3. A flow-type reaction apparatus for continuously reacting two or more kinds of raw material substances, comprising:
a mixing section for mixing two or more of the raw material substances; and
a reaction section provided on the secondary side of the mixing section and obtaining a product by reacting the raw material substances,
the mixing section has: a mixer for mixing two or more of the raw material substances; and two or more supply lines for supplying the respective raw material substances to the mixer,
the supply pipes are respectively connected to the mixers,
at least one of the supply pipes has a suppression mechanism at a connection portion of the supply pipe with the mixer, the suppression mechanism suppressing movement of the fluid from the mixer toward the supply pipe, and at least one of the supply pipes is connected to the mixer from above with respect to a plane in which the mixer is disposed.
4. The flow-type reaction apparatus according to any one of claims 1 to 3, wherein,
the two or more kinds of the raw material substances are a combination of one or more kinds of gas raw materials and one or more kinds of liquid raw materials.
5. The flow-type reaction apparatus according to claim 2 or 3, wherein,
the two or more raw material substances are a combination of one or more gaseous raw materials and one or more liquid raw materials,
at least one of the supply pipes for supplying the gaseous raw material to the mixer is connected to the mixer from above with respect to a plane in which the mixer is disposed, and at least one of the supply pipes for supplying the liquid raw material to the mixer is connected to the mixer in parallel with the plane in which the mixer is disposed.
6. The flow-type reaction apparatus according to any one of claims 1 to 5, wherein,
the reaction device further comprises a separation unit which is provided on the secondary side of the reaction unit and separates a target substance from the product.
CN201880071998.0A 2017-12-05 2018-11-09 Flow type reaction device Pending CN111315474A (en)

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TW201924778A (en) 2019-07-01
WO2019111633A1 (en) 2019-06-13

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